Cleaner Chemical Engineering 3 (2022) 100052

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Cleaner Chemical Engineering

journal homepage: www.elsevier.com/locate/clce

Green solvents, potential alternatives for petroleum based products in food

processing industries
Writdhama Prasad a,∗, Aakash Dadarao Wani b, Kaushik Khamrui c, Shaik Abdul Hussain a,
Yogesh Khetra a
a
Scientist, Dairy Technology Division, ICAR-National Dairy Research Institute, Karnal 132001 (Haryana), India
b
M Tech Scholar, Dairy Technology Division, ICAR-National Dairy Research Institute, Karnal, 132001, (Haryana), India
c
Principal Scientist, Dairy Technology Division, ICAR-National Dairy Research Institute, Karnal, 132001, (Haryana), India

a r t i c l e i n f o a b s t r a c t

Keywords: Solvent extraction is used at the industrial scale for extraction of oil, flavouring and functional compounds from
Solvent extraction the source materials. Easy availability at lower price makes petroleum based solvents (e.g., hexane, petroleum
Green solvents ether, etc.) the preferred choice for solvent extraction. However, some amount of the solvent always escapes
Oil extraction
to the environment during the extraction process and the yield product also contains some amount of residual
herbs and spices processing
solvent. This causes hazard not only to the environment and people at large, but also affects the manpower
Toxicity and environment implications
involved in the solvent extraction industry in particular. This has led to the search of alternative solvents which
have lower toxicity and are environmentally safe. Green solvents appear to be a potential candidate for this.
Solvent extraction studies performed using green solvents have revealed their equal or higher extraction efficacy
to that of petroleum based products. This review paper aims to provide comprehensive information about the
studies pertaining to the application of green solvents as a safer and their potential for replacement of petroleum
based solvents for extraction of fat soluble compounds. In addition, health and environmental aspects of greens
solvents along with their associated advantages-disadvantages has also been discussed in this paper.

1. Introduction
Solvent extraction is encountered during various processes in the
food industry, viz., oil extraction from oilseeds, flavouring and polyphe-
nolic compounds extraction from herbs and spices, etc. According to
Cheng and Rosentrater (2017), about 80% of the cost of oil is con-
tributed by the oilseed itself. This makes the oil extraction more im-
portant, as loss of oil in the residual meal tends to lower the economy
of the plant. In addition of being an economical process for fat extrac-
tion, Zhimin et al (2000) reported that solvent extraction can also be
used to recover residual oil from the pressed oil cake from which oil has
already been extracted using mechanical methods. This indicates about
the vitality of solvent extraction process in the food processing, how-
ever, it comes with certain challenges. Solvents could be considered as
the heart of solvent extraction process for isolation and concentration
of various products (solute) such as oil, flavouring compounds, etc. Be-
cause of ease in availability, petroleum based solvents (such as hexane),
are most commonly used in the food industries for solvent extraction.
However, the European regulation ‘Registration, Evaluation, Authori-
sation and Restriction of Chemicals’ (REACH) has classified hexane as
category 2 reprotoxic and aquatic chronic toxic. Its health hazard has
also been well documented. Agata (2017) reported that long-term ex-
posure of petroleum based solvents may result into harmful effect on
human beings well-being by affecting their respiratory and nervous sys-
tem. This had led to increased concerns about the health of the work-
ers employed in solvent extraction units and on the impact on envi-
ronmental pollution, and led to the search of an alternative to these
petroleum based solvents (Perrier et al. 2017). A potential candidate
as an alternative to these solvents could be the ‘green solvents’. For a
solvent to be considered as ‘green’, it should be derived from renew-
able feedstock which will not remain for long in the environment and
does not lead to the formation of hazardous products during its prepara-
tion or processing (Anastas and Kirchhoff, 2002). As these solvents are
prepared using bio-based materials, they are readily degraded in the en-
vironment and thus are considered as environment friendly and do not
poses human health hazard. Examples of green solvents include ethanol,
cyclopentyl methyl ether, ethyl acetate, 2-methyl tetrahydrofuran (2-
MeTHF), etc. Different studies have been conducted in the recent past
to evaluate these solvents as a potential candidate to replace the conven-
tionally used petroleum based solvents in the food processing industries.

∗
Corresponding author: Scientist, Dairy Technology Division, ICAR-National Dairy Research Institute, Karnal 132001 (Haryana), India. Ph: 0184-2259247; Fax:
0184-2250042.
E-mail addresses: wg.prasad@icar.gov.in, writdhama_3993@rediffmail.com (W. Prasad).

https://doi.org/10.1016/j.clce.2022.100052
Received 1 April 2022; Received in revised form 2 July 2022; Accepted 20 July 2022
2772-7823/© 2022 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/)
W. Prasad, A.D. Wani, K. Khamrui et al.
Fig 1. Flow chart for solvent extraction process
However, a compiled review in this regard is rather scanty, particularly
in the oilseed, herbs and spices extraction industries. Through this pa-
per, we aim to provide comprehensive information about the use of sol-
vent extraction process in oilseed and herbs-spices industries, petroleum
based solvents and their comparison with green solvents in oil, flavour
and functional compounds extraction. We believe that this paper would
be useful for industries involved in solvent extraction and looking for
an alternative to petroleum based solvents.
2. Solvent extraction process
Solvent extraction is a solubility based separation process used to iso-
late the target molecule(s) (solute) from a solid or liquid matrix (source
material) using a suitable solvent. The solvent used for extraction pur-
pose depends on the solubility/polarity of solute to dissolve rapidly in
the solvent and transfer to outside of the source material. The solvent
from solvent-solute mixture is then separated using thermal techniques
such as desolvation, distillation, etc. (Ziaedini et al. 2010). The solvent
extraction process can be classified as liquid-solid and liquid-liquid ex-
traction process with same principle of solvent extraction. A schematic
diagram for the solvent extraction process is summarized in Fig 1. It has
higher separation selectivity and efficacy as compared to other chemical
methods. Further, it has the advantages of economic in operation, large
scale production, fast and continuous in operation. Factors affecting the
solvent extraction efficiency include: (a) Extraction temperature: it has
a direct bearing with the extraction efficacy and an extraction tempera-
ture of 5-10°C (below the boiling point of solvent) is usually employed.
An increase in the extraction temperature results into decrease in the
viscosity and increase in the penetration and solubility of solvent and
solute. However, too high temperature (higher than the boiling of the
solvent) results in gasification (vaporization) and subsequent loss of the
solvent with non-oil substances appearing in the source material. (b) Ex-
traction time: this is important for ensuring that the solvent have enough
2
Cleaner Chemical Engineering 3 (2022) 100052
time to diffuse into the source material and efficiently extract the solute
molecules, but higher extraction time results in high amount of non-
solute molecules in the extract with decreased production capacity. (c)
Solvent: source material ratio: this is important for the fact that a suit-
able amount of solvent (with respect to source material) is required for
penetration and extraction of solutes. A low solvent: source material
ratio have lower extraction efficacy and high solvent: source material
ratio results in the extraction of almost all of the solutes but requires
high energy during the de-solvation process to evaporate the solvent
from solute – solvent mixture. (d) Solvent permeability: this affects the
penetration ability of the solvent inside the source material. Large and
open surface of the source material area enables rapid and permeation
of the solvent and thus the source material are often decompressed or
crushed before solvent extraction (Gaber et al. 2018).
3. Conventional solvents used at industrial scale
Solvents could be considered as the heart of solvent extraction pro-
cess for isolation and concentration of various products (solute) such
as oil, flavouring compounds, etc. at the industrial scale. Johnson and
Lusas (1983) reported that an ideal solvent should be easily removed
from the source material and solute, non-flammable, stable, non-
reactive with oil (solute) or meal (source material) or the equipment,
pure, and easily available at low prices. A brief account of different
petroleum based solvents used for these purposes have been discussed
below and provided in Table 1.
3.1. Hexane
Hexane, a petroleum-derived solvent, has been most widely used
solvent for oil extraction from the oilseeds because of its low boiling
point (69°C), high stability, low corrosiveness, low greasy residual ef-
fect, and an acceptable aroma and flavour profile of the extracted oil
W. Prasad, A.D. Wani, K. Khamrui et al.
Table 1
Physico-chemical attributes of some petroleum based solvents.∗
Solvent n-Hexane Isopropyl alcohol Petroleum ether
Molecular formula C6 H14 C3 H8 O C4 H10 O
Boiling point (°C) 69 82.3 34.6
Molecular weight (g/mol) 86.18 60.1 74.12
Density (25°C, g/cm3 ) 0.675 0.785 0.7134
Viscosity (25°C) 0.31Cp 2.038mPas 0.2448Cp
Flash point (°C) -23 12 -45
∗
Information derived from the material safety data sheet of the respective
solvent of reputed firms.
(Fine et al. 2013). It is an organic compound having six saturated carbon
atoms. It is isolated from gasoline based upon the differences in boiling
point. It is colourless and odourless liquid having high non-polar char-
acter. Because of easy availability and low cost, it is commonly used for
extraction of non-polar compounds. Industrial applications of hexane
include formulation of glues, leather products and extraction of cooking
oils (Castejón, Luna, & Señoráns, 2018).
3.2. Petroleum ether
Petroleum ether is a group of aliphatic hydrocarbons having boiling
point in the range of 40‒80°C. Although it is not classified as ‘ether’,
but the term ‘ether’ is used in its nomenclature to signify its extreme
lightness and volatility. Usually, petroleum ether is provided with a suf-
fix which indicates about it’s boiling range, such as petroleum ether
30–50 indicates that its boiling range is 30–50°C. Commonly available
petroleum ether has suffix 30-50, 40–60, 50–70 and 60–80. This frac-
tionation is important for increasing the selectivity of petroleum ether
as wide boiling range may result in the loss of volatile compounds hav-
ing lower boiling point. It is highly flammable and irritant in nature. It
has been used as solvent for extraction of oil, and in varnish and rubber
industry (Zhou et al., 2019; Anderson, 2019).
3.3. Isopropyl alcohol (IPA)
Isopropyl alcohol (propan-2-ol or isopropanol or 2-propanol) is a
volatile, colourless liquid with sharp musty odour. It has a boiling point
of 82.3°C, which helps in better extraction and solvent-solute mixture
separation. It is can be prepared by two approaches, viz., combining
water and propene (a petroleum based product) or by hydrogenation
of acetone. It is used as an economic solvent during cosmetics, drugs,
shellacs and gums processing (Logsdon & Loke, 2000).
4. Application of solvent extraction in food processing
Extraction is a term used for a process during which the valuable
components are recovered from the source materials by firstly dissolv-
ing them into a liquid (solvent) so that the target compound(s) can be
separated and recovered later from the solvent by using different de-
solvation techniques (Siddique et al. 2020). Solvent extraction can be
encountered during the following processes in the food industry:
i Oil extraction from oilseeds (Table 2).
ii Extraction of flavouring and polyphenolic compounds from herbs
and spices (Table 3).
4.1. Studies on edible oil extraction using petroleum based solvents
The global vegetable oil market was about US$ 96.88 billion in 2019,
which is expected to grow at 3.57% CAGR and attain a value of about
US$ 119.57 billion in 2025 (Researchandmarkets.com). Application of
edible oil in almost all of the cooking operations emphasizes that its
price should be as low as possible so that it is affordable by the com-
mon populace and also profitable to the oilseed industries. According to
3
Cleaner Chemical Engineering 3 (2022) 100052
Cheng & Rosentrater (2017), about 80% of the cost of oil is contributed
by the oilseed itself. This makes the oil extraction process more impor-
tant, as loss of oil in the residual meal tends to lower the economy of the
plant. At a small scale, oil extraction from the oilseeds is performed us-
ing mechanical expression, but solvent extraction is preferred at larger
scale. Cheng (2017) reported that soyabean oil extraction is economical
from solvent extraction using hexane as compared to mechanical ex-
pression, however, Cheng & Rosentrater (2017) reported that an annual
soybean oil production capacity of about 34.64 million kg is required
to make the plant profitable. In addition, Zhimin et al. (2000) reported
that solvent extraction can also be used to recover residual oil from
the pressed oil cake from which oil has already been extracted using
mechanical methods. Gaber et al. (2018) reported that canola cake ob-
tained after mechanical oil expulsion contains about 10-20% oil, which
is recovered by solvent extraction using hexane. However, application
of this method requires a complete refining process to ensure that traces
of the solvents are removed to the maximum extent.
Hu et al. (1996) studied the oil extraction at 60°C for 10min
with 3:1 (solvent: rice bran ratio) using hexane and isopropanol as
the solvents, and reported that oil extraction using isopropanol re-
sulted into higher (6.4%) amount of oil as compared to hexane.
Efeovbokhan et al. (2015) studied oil extraction from Moringa oleifera
seeds grown in northern and southern parts of Nigeria using hexane,
IPA and petroleum ether by varying the extraction time from 2 to 12h.
The authors reported that highest yield (49.38 and 37.57%) was ob-
tained using petroleum ether, followed by hexane (44.94 and 34.71%)
and IPA (36.39 and 28.43%) for northern and southern Moringa oleifera
seeds, respectively. Eganathan et al (2006) compared the oil extrac-
tion efficiency of hexane and petroleum ether from Salicornia brachi-
ate and reported an oil extraction efficiency of 22.40% using hexane
and 10.50% using petroleum ether. Garba et al (2017) has reviewed
the different methods for rice bran oil extraction using hexane as the
solvent. Lakkakula et al (2004) studied the effect of ohmic heating on
rice bran oil extraction efficacy using hexane. The authors observed
that decreasing the frequency of alternating current resulted into an
increase in the amount of extracted oil and reported that applica-
tion of ohmic heating increased the oil extraction efficacy from 53 to
92%. Moreau et al (2003) studied the lipid extraction from ground
corn kernels and rolled oats by pressurized liquid extraction at 40 and
100°C temperatures using hexane, isopropanol, methylene chloride and
ethanol. The authors reported that increasing the solvent polarity and
extraction temperature resulted into an increase in the yield of polar
lipids extraction. Zhang et al (2002) compared IPA at 88, 93, 95 and
97% alcohol concentration with hexane for oil extraction from cotton-
seed flakes and meat using a seven-stage counter-current extraction unit.
The authors reported that 95% alcoholic IPA had higher oil extractabil-
ity from cottonseed collects than flakes, but it was lower than hexane.
Gandhi et al. (2003) compared the soyabean oil extraction efficacy of
hexane, heptane, propanol, IPA and ethanol. The authors reported that
all the studied solvents were equally efficient in extracting the oil with-
out significantly affecting the nutritional attributes (in terms of fatty
acid profile and micro-nutrients) of extracted soybean oil. Amarni &
Kadi (2010) compared the oil extraction efficacy of hexane from olive
cake using soxhlet and microwave assisted solvent extraction method.
The authors reported that in both the extraction methods, increasing
the microwave treatment or heating time-temperature combination in-
creased the oil extraction efficacy; however, the extraction efficacy was
higher in case of microwave assisted extraction as compared to soxh-
let extraction. Fornasari et al. (2017) compared the oil extraction effi-
ciency of petroleum ether and hexane from sunflower (Helianthus annuus
L.), crambe (Crambe abyssinica), peanut (Arachis hypogaea L.), soybean
(Glycine max) and canola (Brassica napus L.) using soxhlet method. The
authors reported that both the solvents yielded similar oil extraction
efficacy (p>0.05) for soyabean (∼17.50%), sunflower (∼37.50%) and
crambe seeds (∼31.00%), but higher oil extraction efficacy was obtained
from petroleum ether for peanut oil (42.44%) and hexane for canola oil
 Table 2
Application of solvent extraction in oilseed processing.

W. Prasad, A.D. Wani, K. Khamrui et al.

Solute (target
Solvent(s) compounds) Source material Processing variables Findings Reference

Isopropyl Alcohol and Cottonseed oil Cottonseed flakes & meat Different concentration of alcohol Hexane had highest oil extraction efficacy, followed by 95% alcoholic Isopropyl Zhang et al. (2002)
Hexane (88, 93, 95 and 97 %) in Isopropyl Alcohol.
Alcohol.
Hexane, Isopropanol, Corn and oat oil Ground corn kernels and rolled Pressurized extraction at 40 and Increasing the solvent polarity and extraction temperature increased the yield of Moreau et al. (2003)
Methylene chloride and oats 100°C temperatures polar lipids extraction.
Ethanol
Hexane Rice bran oil Rice bran Ohmic heating at differing frequency Oil extraction efficacy increased 53 to 92 % with the application of ohmic heating
extraction of alternating current Lakkakula et al. (2004)
Hexane and petroleum Salicornia brachiate Salicornia brachiate seed Seeds dried at 50 °C for 24 hrs and Seed oil had high ester (538.32 mg/g oil) and saponification value (547.52 mg/g Eganathan et al.
ether seed oil ground. oil). (2005)
Seed solvent ratio of 1: 1 Hexane had higher oil extraction efficiency (22.40 %) than petroleum ether (10.50
%).
Hexane Olive oil Olive cake Soxhlet and microwave assisted Increasing the microwave treatment or heating time-temperature combination Amarni &
solvent extraction method increased the oil extraction efficacy. Kadi (2010)
Microwave assisted extraction had higher oil extraction efficacy than soxhlet
extraction method
N-hexane and ethanol Cottonseed oils Cottonseed Solvent: cottonseed ratio of 7:1 Higher oil extraction (68.50 %) using n-hexane as compared to ethanol (65.07 %). Saxena et al. (2011)
Ethanol Rice bran oil Rice bran Different solvent: rice bran: ratio (2.4 Oil extraction efficiency ranged from 42.7 to 99.9 %. Oliveira et al. (2012)
and 4.5: 1) and extraction Oil extraction efficiency increased with increasing extraction temperature and
temperature (60 to 90 °C) solvent: rice bran ratio.
Petroleum ether, hexane Moringa oleifera Northern and southern variety of Extraction time from 2 to 12 hrs. Seed oil yield order: petroleum ether (49.38 and 37.57 %) > hexane (44.94 and
and Isopropyl alcohol seed oil Moringa oleifera seed 34.71 %) > Isopropyl alcohol (36.39 and 28.43 %) for northern and southern Efeovbokhan et al. (2015)
Moringa oleifera seeds, respectively.
Ethyl acetate and hexane Seed oil Canola, flax, mustard and Extraction temperature: 80, 100 and Oil recovery was almost similar for both the solvents and was in the order of canola Lohani et al. (2015)
camelina seeds 120°C; > flax > mustard > camelina.
Extraction time: 40, 65 and 90 min. Optimum oil extraction temperature-time combination of 100°C for 90 minutes
4

using ethyl acetate.

Isopropanol, Fat extraction from Yarrowia lipolytica biomass Maceration for 30 minutes Cyclopentyl methyl ether, ethyl acetate and 2-MeTHF could be used in place of Breil et al. (2016)
d-Limonene, ethanol, Yarrowia lipolytica hexane for oil extraction.
hexane, 𝛼-pinene, ethyl biomass p-cymene, d-Limonene, ethyl lactate, 𝛼-pinene, IPA and ethanol were not suitable
acetate, ethyl lactate, for oil extraction because of lower oil solubility and economic reasons.
di-methyl carbonate,
p-cymene, 2-MeTHF, IPA
and cyclopentyl methyl
ether
Ethanol and Isopropanol Rice bran oil Rice bran Soxhlet method Rice bran oil extracted using aqueous ethanol had 1.53% oryzanol and 769 mg/kg
tocotrienols, while absolute isopropanol extract had higher tocopherol content Capellini et al. (2017)
(98.10 mg/kg).
Petroleum ether and Sunflower oil, Sunflower (Helianthus annuus L.), Soxhlet method Both the solvents had similar oil extraction efficacy for soyabean (∼ 17.50 %),
Hexane crambe oil, peanut Crambe (Crambe abyssinica), sunflower (∼ 37.50 %) and crambe seeds (∼ 31.00 %). Fornasari et al. (2017)
oil, canola oil and Peanut (Arachis hypogaea L.), Higher peanut oil extraction efficacy (42.44 %) was obtained using petroleum ether.
soyabean oil Soybean (Glycine max) and Higher canola oil extraction efficacy (33.68 %) was obtained using hexane.

Cleaner Chemical Engineering 3 (2022) 100052

Canola (Brassica napus L.)
Hexane, dimethyl Oil extraction Litsea cubeba Soxhlet method Dimethyl carbonate and cyclopentyl methyl ether had higher oil extraction efficacy Zhuang et al. (2018)
carbonate, cyclopentyl Oil extracted using dimethyl carbonate and cyclopentyl methyl ether had similar
methyl ether, ethanol fatty acid profile and higher amount of micro-nutrients
and isopropanol.
2-MeTHF and Hexane Black soldier fly oil Black soldier fly (Hermetia Soxhlet method Oil extracted using both the solvents had similar fatty acids profile. Ravi et al. (2019)
illucens) Oil extracted using 2-MeTHF solvent had higher yield and anti-oxidant potential
(total phenolic content of 7.42 mg Gallic Acid Equivalent / gram oil).
2-MeTHF and Hexane Cactus seed oil Cactus seed (Opuntia Ficusindica Seed to solvent ratio of 1:10. Higher oil extraction yield (9.55 ± 0.12 g per 100 g cactus seed) from 2-MeTHF as Gharby et al. (2020)
extraction L.) Extraction time of 8 hrs. compared to hexane (8.86 ± 0.25 g/100 g cactus seed).
2-MeTHF extracted oil was superior in terms of physico-chemical quality indices,
such as acidity, peroxide value and sterol content.
Hexane Copra oil Copra cakes, an agro-industrial Solvent: cake ratio (4, 8 and 12: 1) Increasing the extraction temperature and solvent: cake ratio resulted into higher oil Te et al. (2020)
residue from coconut processing and an extraction temperature of 30, extraction efficacy.
40, and 50°C.
 W. Prasad, A.D. Wani, K. Khamrui et al.
Table 3
Application of solvent extraction in spices and herbs processing.

Solute (target
Solvent(s) compounds) Source material Processing variables Findings Reference

Isopropanol and Hexane Vitamin E and Rice bran Different extraction temperature Increasing the extraction temperature and solvent to bran ratio increased the yield of Hu et al. (1996)
oryzanols (40–60°C) and solvent: rice bran ratio crude rice bran oil, vitamin E and oryzanol.
(2:1 and 3:1). Yield of crude oil and oryzanol was higher in case of isopropanol, and hexane extract
had higher amount of vitamin E.
Ethanol, carbon dioxide Phenolics and Origanum majorana L Soxhelt and supercritical fluid Higher phenolic compounds extraction yield was obtained using ethanol, followed by Vagi et al. (2005)
and Hexane triterpenoid extraction hexane and supercritical fluid extraction.
compounds Order of carnosol concentration in the extract was hexane > supercritical fluid
extraction > ethanol.
Methanol (50 %), Ethyl sage oil Sage Soxhlet extraction Total phenolic content in the sage oil varied from 2,830 to 21,230 mg per 100 g. Akkol et al. (2008)
acetate and Hexane Order of extraction efficacy was found to be: 50 % methanol > pure methanol > ethyl
acetate > hexane.
Ethanol and carbon Flavonoid Spearmint (Mentha spicata L.) Soxhlet and supercritical fluid Higher crude extract yield (257.67 mg/g) was obtained using Soxhlet extraction than Bimakr et al. (2011)
dioxide extraction supercritical fluid extraction (60.57 mg/g)
Extract obtained using supercritical fluid extraction had higher number of bioactive
flavonoids (# 7) in comparison to Soxhlet method (# 5).
Hexane and carbon Oleoresin Paprika Soxhlet and supercritical fluid Higher amount of pigments were obtained in hexane extract
dioxide extraction. Supercritical fluid extract had higher amount of 𝛼-tocopherol content (3846.9 mg/kg). Saponjac et al. (2014)
5

Hexane, Ethanol, umbelliferone and Matricaria chamomilla Soxhlet extraction using hexane, Order of umbelliferone and herniarin yield: maceration (20.85 %) > soxhlet (4.60 %) Molnar et al. (2017)
supercritical fluid and herniarin maceration using 50 % aqueous > super critical fluid extraction (1.57 %) > hydro-distillation (0.41 %).
water ethanol, super critical fluid extraction
and hydro-distillation.
Ethanol Polyphenolic Pomegranate peel Solvent: peel ratio of 15 and 60: 1 Increasing the solvent: peel ratio increased the polyphenols extraction. Sandhya et al. (2018)
compounds Ethanolic extract had higher amount of polyphenols than aqueous extract.
Petroleum ether Coffee oil Roasted coffee beans Soxhlet (200 mL and time 480 Similar yields (∼ 16 %) were obtained in both the processes; Pinto et al. (2019)
minutes) and pressured solvent Extraction using pressurized solvent system requires less amount of solvent (20 mL)
extraction (solvent 20 mL and time and time (20 minutes).
20 minutes) for 8 grams of roasted
coffee beans.
Hexane Phenolic compounds Moringa peregrine seeds Soxhlet (11hrs extraction) and Highest yield of oil extraction (53.10 %) was obtained at liquid to solid ratio of
from Moringa ultrasound-assisted extraction method 17.8 mL/g for 26.30 minutes of extraction time. Mohammadpour et al.
peregrine seeds (liquid: solid ratio 5-20 mL/g and an Oil obtained through ultrasound-assisted extraction possessed superior polyphenolic (2019)
extraction time of 5 to 30 minutes content and anti-oxidant attributes.
were studied at an ultrasound power

Cleaner Chemical Engineering 3 (2022) 100052

of 348 W and 30°C temperature).
Ethanol, Ethyl acetate Phenolics and Garlic (Allium sativum) Extraction durations: 35, 50 and 65 Methanolic extract obtained after 50 minutes of extraction time had highest amount of Awan et al. (2019)
and Hexane flavonoid extract minutes phenolics (60.38±0.23 mg GAE/100g) and flavonoids (58.45±1.24 mg/100g) content.
p-cymene Bitter gourd seed oil Bitter gourd seed Ultrasound assisted, microwave Order of oil yield: microwave assisted extraction (30.42 %) > ultrasound assisted Naik et al. (2021)
assisted and ohmic assisted extraction (27.42 %) > ohmic assisted extraction (25.34 %).
extraction. Oil extracted using ultrasound contained higher levels of poly-unsaturated fatty acids.
W. Prasad, A.D. Wani, K. Khamrui et al.
(33.68%). Te et al. (2020) reported about lipid extraction from Copra
cake, an agro-industrial residue from coconut processing, using hexane
as the solvent. The authors first acid hydrolyzed the Copra cake, followed
by subjecting it to solvent: cake ratio (4, 8 and 12:1) and an extraction
temperature of 30, 40, and 50°C and reported that increasing the extrac-
tion temperature and solvent: cake ratio resulted into an increase in the
oil extraction yield.
4.2. Application in spices and herbs processing
Flavour is an important sensory impression and greatly affects the
acceptability of food products. Flavour arises as a result of a mixture
of volatile aroma compounds and can be classified as natural, natural
identical and artificial flavouring compounds. These flavour compounds
could be developed within the product (in situ) during the course of
product preparation and/or can be added into the product from ex-
ternal sources (ex situ). However, direct addition of herbs and spices
into food products as a source of flavour (or functionality) is also ac-
companied with the change in color and appearance attribute of the
product; hence, flavour compounds are generally first isolated from the
herbs and spices and then added into the food product. This approach
also increases the stability of flavour active compounds. These flavour-
active components are widely used in beverage industry with the largest
market in North America, followed by Asia-pacific and Europe. As per
the data available from alliedmarketresearch.com (2021), global mar-
ket size of the flavour industries was $14.6 billion in 2019, which is
expected to grow at 4.60% CAGR and reach $17.4 billion by 2027. In
addition, growing health awareness of the common populace at large
has resulted into a huge market for functional foods. Functional foods
may be defined as foods which provide health benefits beyond the basic
nutrition. Addition of herbs or herbal extract tends to increase the func-
tionality of the product, besides affecting the flavour and other sensory
profile of the product (Meena et al., 2021a&b). Functionality of herbs
and spices is primarily associated with the polyphenols present in them.
The polyphenols, besides increasing the functionality, also increases the
stability of the product by possessing anti-microbial and anti-oxidant ac-
tivity. Kumbhare et al. (2021) reported about use of different solvents,
viz., ethanol, chloroform, ethyl acetate, water, etc. for the extraction
of polyphenols from different sources (viz., rice bran, fruit peels, etc.)
for increasing the shelf life and functionality of ghee, clarified butter
fat. Wani et al. (2022a&b) reported about the use of different solvents,
like dichloromethane and water, for processing of ghee residue, clarified
butter sediment waste. Similarly, Badola et al. (2022) reported about
the use of polyphenol extracted using different solvents for increasing
the functionality and shelf life of milk based sweetmeats. This indicates
about the use of solvent extracted polyphenols in different products.
Extraction of polyphenols from their source material is performed using
different solvents. A brief account of use of different petroleum based
solvents for the extraction of polyphenols from the herbs-spices is dis-
cussed below.
Monsálvez et al. (2010) studied the anti-fungal activity of Drimys
winteri extract obtained using hexane. For obtaining the extract, 2L of
hexane was mixed with 700g of dry bark and left for maceration (24h),
followed by filtration of the contents and evaporation of hexane from
the filtrate using Rotavapor at 35°C temperature and 0.3bar pressure.
The authors reported that the anti-fungal compounds present in the ex-
tract were drimenin, drimenol, polygodial and isodrimenol. Also, appli-
cation of the extract at 250mg/kg level decreased the severity of fungal
damage and has a protecting effect on the growth of wheat seedlings
caused by Gaeumannomyces graminis. Saponjac et al. (2014) compared
the Paprika oleoresins extraction using soxhlet (hexane as solvent) and
supercritical fluid extraction. The authors reported that higher amount
of pigments were obtained in hexane extract, while supercritical fluid
extract had higher amount of 𝛼-tocopherol content (3846.9mg/kg).
Ahmed et al (2018) studied the extraction of essential oil from Corian-
drum sativum using different solvents and reported that highest yield
6
Cleaner Chemical Engineering 3 (2022) 100052
(8.82%) was obtained from petroleum-ether, followed by chloroform
(7.07%) and methanol (6.72%). Pinto et al. (2019) studied the coffee
oil extraction from roasted coffee beans using petroleum ether through
soxhlet and pressured solvent extraction. The authors reported that sim-
ilar yields (∼16%) were obtained in both the processes; however, ex-
traction using pressurized solvent system requires less amount of sol-
vent (20mL) and time (20min) as compared to soxhlet system (200mL)
and time (480min) for the same amount (8g) of roasted coffee beans.
Molnar et al. (2017) studied the extraction of umbelliferone and her-
niarin from Matricaria chamomilla using different techniques, viz., soxh-
let extraction using hexane, maceration using 50% aqueous ethanol,
super critical fluid extraction and hydro-distillation. The authors re-
ported that the yield of umbelliferone and herniarin was in the or-
der of maceration (20.85%) > soxhlet (4.60%) > super critical fluid
extraction (1.57%) > hydro-distillation (0.41%). Umamaheshwari &
Reddy (2016) studied the solvent extraction of dried bitter gourd seeds
using n-hexane and reported a yield of 51% at 100°C extraction temper-
ature for 150 min. Kanadea & Bhatkhandeb (2016) studied the ginger
oil extraction using acetone and reported that an extraction temperature
of 80°C for 60 min was optimum for ginger oil extraction from fresh gin-
ger. Mohammadpour et al. (2019) compared the extraction of phenolic
compounds from Moringa peregrine seeds using hexane through soxh-
let and ultrasound-assisted extraction method. During the ultrasound-
assisted extraction, liquid:solid ratio 5-20mL/g and an extraction time
of 5 to 30 min were studied at an ultrasound power of 348W and 30°C
temperature. The authors reported that highest (53.10%) yield of ex-
tract (oil) through ultrasound-assisted extraction was obtained at liquid
to solid ratio of 17.8 mL/g for 26.30 min of extraction time, while ex-
traction through soxhlet method had an yield of 43% after 11h of ex-
traction. Also, the oil obtained through ultrasound-assisted extraction
possessed superior polyphenolic content and anti-oxidant attributes.
Rose et al. (2021) studied the oil extraction efficiency and lipid classes of
oil extracted from insect powders using hexane, chloroform, methyl-tert-
butyl ether (MTBE), and 3:2 ratio hexane-isopropanol and compared
them with a solvent mixture comprising of chloroform-methanol (CM)
in 2:1 ratio. The authors reported that oil extraction efficacy was highest
using CM for adult cricket and locust insect, while MTBE had the highest
efficacy for silkworm pupae insect. In addition, all the solvent extracted
oil had similar (p>0.05) lipid classes. These studies clearly indicate that
petroleum based solvents have widespread applications in the extraction
purposes in food industry. At times their extract also contains higher
amount of anti-oxidants, but it should also be considered that these sol-
vents have detrimental effects on the human health as well as on the
environment. Studies conducted on the environmental and toxic effects
of petroleum based solvents have highlighted the need to move towards
greener alternatives.
5. Environmental and health impacts of petroleum based solvents
From the information provided in the previous section, it is clear that
solvent extraction is used for the extraction of oil, flavour and polyphe-
nolic compounds during food processing. But the residual solvent that
is present in the final extract is always a cause of concern to the food
industries. According to Food Safety and Standards Authority of India
(FSSAI), a regulatory body of Indian government dealing with the safety
of food products, a maximum of 5mg/kg of hexane has been allowed as
residual solvent in the oils obtained using solvent extraction, and such
product must contain a label as ‘solvent extracted oil’ on the package
to ease in costumers’ information. Similarly, the European regulation
‘Registration, Evaluation, Authorisation and Restriction of Chemicals’
(REACH) has categorized hexane as category 2 reprotoxic and aquatic
chronic toxic (Sicaire et al. 2015). Concerns about the negative health
implications of exposures of these petroleum based solvents have also
been in debate in the recent times. Organic solvents pose a potential
health and environment hazard primarily because of their volatile na-
ture. Applications of petroleum based solvents in the food industry have
W. Prasad, A.D. Wani, K. Khamrui et al.
increased concerns about the health of operators and impact on environ-
mental pollution (Perrier et al. 2017). During solvent extraction, separa-
tion of the desired compound from solvent is performed by the evapora-
tion of volatile solvent. Exposure of these solvents to workers present in
the extraction area may result into irritation and problems in their neu-
ral system (Kumar et al. 2017). Short term exposure of these solvents
leads to nausea and dizziness; while the long term exposure might lead
to malfunctioning in liver, kidney and even in the central nervous sys-
tem (Crinnion, 2010). Similarly, Agata (2017) reported that long-term
exposure of petroleum based solvents may result in harmful effect on
human beings well-being by affecting their respiratory and nervous sys-
tem. According to WHO, about one-fourth of diseases arise as a result of
long-term exposure of environmental pollutants. Jutz et al. (2011) re-
ported that each year, more than twenty million tons of waste residues
from organic solvents are emitted to the atmosphere that results into
unnecessary wastage of solvents and pollution of the environment. This
highlights of the urgency to look for alternative solvents which could
extract the compound(s) of interest as like the conventional petroleum
based solvents without having detrimental effects on the human health
and environment.
6. Green Solvents
Rising awareness about the detrimental effects caused by the
petroleum based solvents has emphasised on the need for sustainable
development strategies that should address the health and environmen-
tal impact without compromising the extraction yield and quality of
extract during the solvent extraction process. Legislations are made in
different countries to restrict the food applications of these petroleum
based solvents, such as European Union passed ‘Directive 2009/32/EC’
in 2009 for restricting the food applications of toxic solvents. Similarly,
amendments were made in the ‘Clean Air Act’ of USA in the year 1990
relating to the environmental and health concerns of hexane, which
led to the search of alternative solvents (Gandhi et al. 2003). Accord-
ing to Anastas and Williamson (1996), green organic processes should:
(a) avoid waste generation and be energy efficient, (b) avoid the use
or generation of harmful and toxic chemicals, (c) use biodegradable,
environment friendly chemicals or solvents and renewable materials.
‘Green solvent’ concept was derived from the ‘green organic processes’
and was summarized by Anastas and Kirchhoff (2002). For a solvent
to be considered as ‘green’, it should be derived from renewable feed-
stock which will not remain for long in the environment and formation
of hazardous products during its preparation or processing should be
avoided (Anastas and Kirchhoff, 2002). As they are prepared from bio-
based materials that are readily degraded in the environment, they are
environment friendly and do not possess human health hazard. Exam-
ples of green solvents include ethanol, cyclopentyl methyl ether, ethyl
7
Cleaner Chemical Engineering 3 (2022) 100052
Fig 2. Green solvents covered in the present review
acetate, 2-MeTHF, etc. (Fig 2). Watanabe et al (2007) reported that cy-
clopentyl methyl ether is being encouraged as a green solvent for adop-
tion at the industrial scale by the American Chemical Society because of
its desirable oil solubility and higher stability under processing condi-
tions. Pace et al (2012) reported 2-MeTHF as a green solvent because of
the fact that it could be derived from the cellulose present in agricultural
biomass such as corncobs, sugar cane bagasse, oat hulls, etc. and it is de-
graded by the exposure of sunlight and air. Similarly, ethanol, which is
produced during anaerobic fermentation of sugarcane bagasse, has also
been used for solvent extraction as a greener alternative to petroleum
based solvents. Considering the health hazard associated with petroleum
based solvents, FSSAI has also allowed the use of ethanol and its aque-
ous solution for the extraction of polyphenolic compounds from herbs
and spices under Food Safety and Standards Regulations (2016). The fol-
lowing section deals with the studies pertaining to use of green solvents
in the extraction of oil, flavouring and polyphonic compounds from the
source materials.
6.1. Applications of green solvents in food industries
6.1.1. Application in oil extraction
Saxena et al (2011) compared the extraction efficacy of cottonseed
oil using n-hexane and ethanol and reported that the solvent to solid
ratio of 7:1 was optimum for both solvents to extract the maximum
amount of oil. Also, higher yield was obtained using ethanol (68.50%)
as compared to hexane (65.07%). Oliveira et al (2012) studied the oil
extraction efficiency using ethanol at different solvent: rice bran ratio
(2.4 and 4.5:1) and extraction temperature (60 to 90°C). The authors re-
ported that the oil extraction efficiency ranged from 42.7 to 99.9%, and
the oil extraction efficiency increased with an increase in the extrac-
tion temperature and solvent: rice bran ratio. Ying et al (2013) com-
pared the rapeseed oil extraction efficacy of hexane with ethanol, iso-
propanol and terpenes. The authors reported that hexane could be re-
placed by p-cymene (terpene) because of its high lipid yield and se-
lectivity as the extract obtained using p-cymene (terpene) had higher
amount of polar lipids and lower levels of tocopherol and tocotrienol.
Lohani et al (2015) compared the oil extraction efficacy of ethyl ac-
etate with hexane from canola, flax, mustard and camelina seeds. The
authors kept solvent: seed ratio at 4:1 and varied the extraction tem-
perature (80, 100 and 120°C) and time (40, 65 and 90min). Oil recov-
ery was almost similar for both the solvents and was in the order of
canola > flaxseed > mustard > camelina. Except density and viscosity
(higher in case of ethyl acetate extracted oil), all other quality param-
eters of the oils extracted using both the solvents were almost identi-
cal. The authors recommended an extraction temperature-time combi-
nation of 100°C for 90 min for oil extraction from the studied oilseeds
using ethyl acetate. Sicaire et al (2015) studied the edible oil extraction
W. Prasad, A.D. Wani, K. Khamrui et al.
efficacy of 2-MeTHF as a substitute for hexane from rosemary seeds.
The extraction was carried out at 1:5 (solvent: rosemary seed ratio) for
8h at 55°C. The authors reported that the 2-MeTHF extract contained
higher amount of tocopherols, sterols and tocotrienols, in addition to
the triglycerides. Breil et al (2016) compared the feasibility of fat ex-
traction from Yarrowia lipolytica biomass using different solvents, viz.,
isopropanol, d-Limonene, ethanol, hexane, 𝛼-pinene, ethyl acetate, ethyl
lactate, di-methyl carbonate, p-cymene, 2-MeTHF, IPA and cyclopentyl
methyl ether by maceration for 30 min. The authors reported that cy-
clopentyl methyl ether, ethyl acetate and 2-MeTHF could be used in
place of hexane for their ability to efficiently solubilise the microbial oil
at similar energy requirement and carbon emission, on the other hand,
p-cymene, d-Limonene, ethyl lactate, 𝛼-pinene, IPA and ethanol were
not suitable for oil extraction from Yarrowia lipolytica biomass because
of lower oil solubility and economic reasons. Capellini et al (2017) used
ethanol and isopropanol in rice bran oil extraction with an aim of re-
placing hexane with safer solvents. The authors reported that aque-
ous nature of alcoholic solvents negatively affected the oil extraction
efficiency. Rice bran oil extracted using aqueous ethanol had 1.53%
oryzanol and 769mg/kg tocotrienols, while absolute isopropanol extract
had higher tocopherol content (98.10mg/kg) as compared to other sol-
vents. The authors concluded that short chain alcohols could serve as
better alternatives to hexane for solvent extraction of oil from oilseeds.
Zhuang et al (2018) compared the oil extraction of hexane from Litsea
cubeba with four solvents, viz., dimethyl carbonate, cyclopentyl methyl
ether, ethanol and isopropanol. The authors reported that dimethyl car-
bonate and cyclopentyl methyl ether had higher oil extraction efficacy
than ethanol and isopropanol. In addition, oil extracted using dimethyl
carbonate and cyclopentyl methyl ether had similar fatty acid profile
and higher amount of micro-nutrients as compared to that of hexane.
Ravi et al (2019) compared the oil extracted from black soldier fly (Her-
metia illucens) using 2-MeTHF and hexane. The authors reported that
oil extracted using both the solvents has similar fatty acids profile, but
2-MeTHF solvent had higher yield and anti-oxidant potential (total phe-
nolic content of 7.42mg Gallic Acid Equivalent/gram oil), which indi-
cated about the higher stability of 2-MeTHF extracted oil as compared
to hexane extracted oil. Gharby et al (2020) studied the lipid extrac-
tion behaviour of 2-MeTHF from cactus seed (Opuntia Ficusindica L.).
The authors reported an extraction yield of 9.55±0.12g per 100g cactus
seed from 2-MeTHF, which was higher than those obtained from hexane
(8.86±0.25g/100g). Also, the 2-MeTHF extracted oil was superior than
hexane extracted oil in terms of physico-chemical quality indices, such
as acidity, peroxide value and sterol content.
6.1.2. Application in herbs and spices processing
In the mid-1990s, Miller (1995) isolated 21 semi-volatile flavour
compounds from cinnamons using ethyl acetate through supercritical
fluid extraction. Hu et al (1996) studied the vitamin E and oryzanols
extraction efficiency of isopropanol and hexane from rice bran at dif-
ferent extraction temperature, time and solvent: rice bran ratio. The au-
thors reported that increasing the extraction temperature from 40 to
60°C and solvent (hexane and isopropanol) to bran ratios of 2:1 and
3:1 resulted in an increase in the yield of crude rice bran oil, vita-
min E and oryzanol in the extracted oil. Also, the yield of crude oil
and oryzanol was higher in case of isoproponol, and hexane extract had
higher amount of vitamin E. Vagi et al. (2005) reported about the ex-
traction of phenolics and triterpenoid compouds from Origanum majo-
rana L. using ethanol, hexane and supercritical fluid extraction. The au-
thors reported that higher extraction yield was obtained using ethanol,
followed by hexane and supercritical fluid extraction, but the order of
carnosol concentration in the extract was hexane > supercritical fluid ex-
traction > ethanol. Akkol et al (2008) extracted sage oil using different
solvents and reported that the total phenolic content in the sage oil var-
ied from 2,830 to 21,230 mg per 100 g. Order of extraction efficacy was
found to be: 50% methanol > pure methanol > ethyl acetate > hexane.
8
Cleaner Chemical Engineering 3 (2022) 100052
Peev et al (2011) used ethanol-water mixture {50:50 and 80:20 (v/v)}
for rosmarinic acid extraction from dry lemon aerial parts and reported
a recovery of about 94%. Bimakr et al (2011) compared the flavonoid
extract of spearmint (Mentha spicata L.) obtained using conventional
soxhlet method (aqueous ethanol solvent) and supercritical fluid extrac-
tion (carbon dioxide). The authors reported that higher crude extract
yield (257.67mg/g) was obtained using soxhlet extraction than super-
critical fluid extraction (60.57mg/g), but the extract obtained using su-
percritical fluid extraction had higher amount of bioactive flavonoids
(#7 viz., catechin, epicatechin, rutin, myricetin, luteolin, apigenin and
naringenin) in comparison to soxhlet method (#5 viz., catechin, epi-
catechin, rutin, luteolin and apigenin). Akintobi et al (2016) studied
extracted polyphenols from Parkia biglobosa (a medicinal tree found in
Africa) root bark using water, ethanol, petroleum ether and hexane, and
studied their anti-microbial activity at 40mg/mL level. The authors re-
ported that the extract obtained using ethanol had antimicrobial activity
against all the studied pathogens, while hexane extract had inhibitory
effect only against Klebsiella pneumoniae. Further, the authors reported
that the root bark had alkaloids, terpenoids, steroids, flavonoids, tan-
nins, saponins, phlobatannins and anthraquinones, among which an-
thraquinones could not be extracted by any of the studied solvents.
Sandhya et al (2018) extracted polyphenols from pomegranate peel
using aqueous and ethanol solvent at solvent: peel ratio of 15 and
60:1. The authors reported that increasing the solvent: peel ratio in-
creased the polyphenols extraction, and in both the studied solvent:
peel ratio, ethanolic extract had higher amount of polyphenols than
aqueous extract. Awan et al (2019) compared the extraction efficacy
of ethanol, ethyl acetate and hexane at different extraction durations
(35, 50 and 65 min) for obtaining garlic (Allium sativum) extract and
reported that the methanolic extract obtained after 50 minutes of ex-
traction time had highest amount of phenolics (60.38±0.23 mg Gal-
lic Acid Equivalent/100g) and flavonoids (58.45±1.24 mg/100g) con-
tent. Naik et al (2021) studied the extraction of bitter gourd seed oil
through ultrasound assisted, microwave assisted and ohmic assisted
extraction using p-cymene as a green solvent. The authors reported
that highest oil yield was obtained by microwave assisted extraction
(30.42%), followed by ultrasound assisted extraction (27.42%) and
ohmic assisted extraction (25.34%), and the oil extracted using ultra-
sound contained higher levels of poly-unsaturated fatty acids. Recently,
Torgbo et al. (2022) used deionized water and ethanol for extraction of
polyphenols from rambutan peel using ohmic heating. The authors re-
ported that gallic, corilagin, geraniin and ellagic acid were the major
phenolic compounds present in the extract and ethanolic extract had
higher yield of polyphenols as compared to deionized water. Also, the
authors used this extract for increasing the shelf life of bread and re-
ported that the extract exhibited anti-fungal activity in bread and re-
sulted into an increase in its shelf life from 3 to 7 days.
These studies clearly indicate that green solvents could be used as
an alternative to petroleum based solvents for extraction purposes in
the food industry, be it oil extraction or functional and flavouring com-
pounds extraction from herbs and spices. However, most of the indus-
tries still rely on petroleum based solvents for extraction activities. This
could probably be due to lesser awareness about the extraction efficacy
of the green solvents. Further, availability of these solvents at compet-
itive prices with the conventional solvents is also a concern. In addi-
tion, information pertaining to the level of residual green solvent present
in the extracted product, toxicological studies of the solvent extracted
product and their comparison with the conventionally extracted prod-
uct, and most importantly the difference in the net environment impact
by switching from petroleum based solvents to green solvents needs
to be comprehensively determined and quantified under the practical
conditions. This will not only provide a strong database (regarding the
safety and environmental implications of green solvents) to the govern-
ment agencies for framing suitable legislations, but will also encourage
the industries to migrate towards green solvents.
W. Prasad, A.D. Wani, K. Khamrui et al.
7. A deeper insight into the green solvents
7.1. Are green solvents actually green?
The previous section provided that green solvents could also be used
as a replacement for petroleum based products in food industries for
different extraction purposes. However, it is important to mention that
before being used at a commercial scale, the green solvent must be ac-
cessed for various parameters, including the economic ones. Eventually,
the process should be economical so that the final product is affordable
to the consumers at large. In addition, the production of green solvents
should not be detrimental to the environment as they should not lead
to or rely upon toxic compounds during their production or recycling.
Although green solvents (particularly the bio-based solvents) rely upon
agricultural sources for their production, but the agricultural commodi-
ties have a continuous fibrous structure containing numerous classes of
compounds. This necessitates for their prior processing (sometimes us-
ing toxic chemicals) in order to use them for solvent production. Further,
the process for production of some green solvents relies on hazardous
compounds. For instance, 2-MeTHF is produced from agricultural com-
modities rich with lignin, cellulose and hemicelluloses (such as corncobs
and sugarcane bagasse) by the hydrogenation of furfural (Chemat et al.,
2019). Furfural, produced by sulphuric acid treatment of pentose (C5)
sugars, is known to cause irritation to skin, mucous membrane and res-
piratory tract. Similarly, DMC can be produced through different ways,
viz., through Bayer’s process using carbon-monoxide; methanolysis of
urea (with the generation of ammonia, a toxicant and pollutant, as by-
product); reaction of methanol with carbon(IV)oxide, propylene car-
bonate, ethylene carbonate, phosghene (a highly toxic gas); or from
methyl nitrite process (Esan et al., 2020). Cyclopentyl methyl ether can
be produced in two ways, viz., methylation of the cyclopentanol (an ir-
ritant) or by the addition of methanol to the cyclopentene (an irritant)
(Chemat et al., 2019). However, relying on toxic chemicals or gener-
ation of toxic chemicals as a by-product is not true for all the green
solvents. For examples, production of ethanol can be done through the
fermentation of bagasse using certain micro-organisms, viz., S. cerevisiae,
L. fermentum, etc. Similarly, ethyl acetate can be produced by esterifica-
tion of ethanol and acetic acid. Terpenes can be produced using steam
distillation of dried plant resources. This indicates of the fact that al-
though bio-based solvents have agricultural origin, yet their associated
toxic and environmental effects vary for the individual solvent. Further,
relying/generation of the toxic chemicals also do not mean that these
solvents are equally hazardous as like the petroleum based counterparts.
According to Gu and Jérôme (2013), green solvents should be evaluated
on 12 different parameters related to biodegradability, toxicity, renewa-
bility, availability, production, compatibility, etc. This appears to be a
more comprehensive evaluation as it not only differentiates petroleum
based solvents from others, but also enables easy segregation of bio-
based green solvents based upon their production and other character-
istics. It is further important to mention here that through these pa-
rameters, 2-MeTHF appears less greener than ethanol but it is more ef-
ficient in oil extraction (Breil et al., 2016). On similar lines, water is
considered as a green solvent satisfying almost all of the parameters
stated by Gu and Jérôme (2013), yet it is not suitable for fat extraction
from oilseeds. This emphasizes on the need to look for less hazardous
(and greener) alternative than the existing ones so that the solvent re-
mains compatible with the solute and does not severely affect the ex-
traction economics. Considering this approach takes care of the greener
alternatives along with economics of the extraction process (Häckl and
Kunz, 2018).
Further, comparison of the toxicity data for LD50 (oral and dermal)
and LC50 (inhalation) in animal models from the material data safety
sheet (MSDS) of the respective solvent revealed that some of these green
solvents have similar toxicity as that of hexane, IPA and petroleum ether
(Table 4). This appears contradictory because at one point it is being em-
phasized that green solvents (particularly the bio-based ones) are envi-
9
Cleaner Chemical Engineering 3 (2022) 100052
ronment friendly and yet they have similar toxicity as that of petroleum
based solvents. This ambiguity could be attributed to the easy degrad-
ability in the environment and lower environmental impacts of the green
solvents. For example, Life cycle assessment (LCA) is performed to eval-
uate the environmental impacts of a chemical during its life i.e., from
production to consumption/end use. It has been commonly employed to
compare the environmental impacts of different chemicals and for selec-
tion of an environment friendly material. Potrich et al (2020) compared
the environmental impact and economics for replacement of hexane by
ethanol for the extraction of soybean oil. The authors reported that soy-
abean oil extraction was economical through both the solvents, but hex-
ane presented a higher (10.2%) economy as compared to ethanol. On
the other hand, ethanol as a solvent had low global warming potential
by decreasing the CO2 equivalent production of about 10600 tonnes per
year by an industry of 125 ton per hour soybean processing capacity. On
similar lines, Cheng et al. (2018) compared the environmental impact
of soyabean oil production using conventional processes, viz., solvent
extraction using hexane and mechanical processing of soyabean seeds,
and compared them with a novel enzyme assisted extraction processing
(EAEP) using water as a solvent. It was observed that solvent extraction
using hexane had the highest environmental impact; mechanical press-
ing had the highest production of greenhouse gases (GHG) because of
high energy requirement. Environmental impact of mechanical press-
ing process was similar to that EAEP but the later had lower GHG and
pollutants emission.
In addition to comparison of environmental impact of different
chemicals, LCA has also been used to compare the environmental
impact of different processes for the production of same chemical
from different sources/techniques. Previously, it was stated that 2-
MeTHF is produced using agricultural biomass through acid hydrol-
ysis to obtain furfural, which is subsequently treated to produce 2-
MeTHF. Slater et al. (2016) compared the LCA for manufacturing of
2-MeTHF using biogenic and non-biogenic sources and reported that
biogenic source resulted into 97% reduction in emission (0.191kg, in-
cluding 0.150kg CO2 ) for production of 1 kg 2-MeTHF. Aresta and
Galatola (1999) reported that DMC production from phosgene had
four times higher environmental impact as compared to CO2 . Garcia-
Herrero et al. (2016) compared the environmental impact of DMC pro-
duction from conventionally used oxidative carbonylation of methanol
with a newly developed electrochemical method using CO2 as the raw
material. The authors reported that electrochemical process produced
63.3 to 94.5 kg CO2 equivalent per kg of DMC, which was 25 times
higher than the conventional process (3.2 kg CO2 equivalent per kg
DMC). This was because of the lower yield (0.7%) in the developed pro-
cess and recommended that the yield must be increased to 20% to make
it at par with the conventional process. Methanol, an intermediate ma-
terial required for the production of DMC and cyclopentyl methyl ether,
can be produced using different sources, viz., fossil fuels (coal, crude
oil and natural gas) and agricultural biomass. Among them, majority of
methanol is produced using coal as the raw material. This results into
generation of huge amount of pollutants such as oxides of nitrogen and
sulphur. Chen et al. (2019) evaluated the LCA of methanol production
from different sources and reported that methanol production from coal
had 2.0 to 3.4 times higher environmental impact as compared to using
coke oven gas and natural gas as the raw material. Further, the authors
reported that electricity was found to be the most important factor in
determining the environmental impact of methanol production through
these raw materials. After considering electricity from clean source, the
environmental impact could be reduced by 83.5, 82.2 and 66.5% for
methanol production from natural gas, coal, and coke oven gas, respec-
tively. These findings clearly indicate that the green solvents have com-
paratively lesser environmental impact as compared to the petroleum
based solvents. Search for a clearer process to prepare these solvents
will further aid in decreasing the carbon emissions and moving towards
a greener system. Further, more information is needed pertaining to en-
vironmental impact of these solvents from different extraction indus-
W. Prasad, A.D. Wani, K. Khamrui et al. Cleaner Chemical Engineering 3 (2022) 100052

Table 4
Toxicity information∗ of green and petroleum based solvents.

LD50 Dermal LC50 inhalation

LD50 Oral (mg/kg) (mg/kg) (ppm/m3 /4h) Flammability hazard Health hazard

Green solvents
DMC 13000 (rat) >5000 (rabbit) >140 (rat) Category 2 Category 2
2-MeTHF 300-2000 (rat) 4500 (rabbit) 6000 (rat) Category 2 Category 4
Methanol 5628 (rat) 15800 (rabbit) 1307 (rat) Category 2 Category 3
Ethanol 7060-9000 (rat) 20000 (rabbit) 117-125 (rat) Category 2 Category 2
Ethyl acetate 10200 (rat) > 18000 (rabbit) 200 (8h) (rat) Category 2 Category 3
Cyclopentyl methyl 200-2000 (rat) > 2000 (rat) > 21.5 (rat) Category 2 Category 4
ether
Petroleum based solvents
n-Hexane 25 000 (rat) 3000 (rabbit) 48000 (rat) Category 3 Category 1
Isopropyl alcohol >90 (rat) 3600 12800 (rabbit) 16000 (8 h) (rat) Category 2 Category 3
(mouse)
Petroleum ether Not available Not available 3400 (rat) Category 1 Category 1

LD50 oral: Dosage of a substance, given at once, that can be expected to be lethal for 50% of the animals in a dose group.
LD50 dermal: Statistically derived single dose of a substance that can be expected to be lethal in 50 per cent of treated animals when
applied to the skin.
LC50 inhalation: Concentrations of the substance in the air that can be expected to be lethal to 50% of the test animals during the
observation period (usually 4-8 h).
∗
Information derived from the material safety data sheet of the respective solvent of reputed firms.

tries. In addition, toxicological studies of the solvent extracted products
also need to be carried out to have an evidence of the health implications
of products extracted using green solvents.
7.2. Advantages-Disadvantages associated with green solvents
Undoubtedly, green solvents appear to be advantageous over
petroleum based solvents for their bio-based origin. This corresponds to
economical utilization of agricultural residues for income generation,
and reduced load on waste management system and stable burning re-
sulting into lesser generation of pollutants and air pollution. In addition
to these, it also decreases the environment pollution by rapid degrada-
tion, superior quality products as the residual solvent in the product is
relatively lesser harmful to the consumer as compared to the petroleum
based solvents. It also paves the way for migration from dependence on
a limited stock of fossil fuels to renewable source of agricultural com-
modities as the raw material. Use of solvents like ethanol, supercritical
CO2 , etc. also results into improving the safety of workers involved in
the solvent extraction process.
While some of the green solvents (like CO2 , water, etc.) are easily
available and inexpensive, but the major disadvantage for using the re-
maining green solvents could be related to their increased cost and thus
the cost of final product. Easy availability of the petroleum based sol-
vents provides them an added advantage over the green solvents, this is
particularly true for the non-polar solvents. It was reported in the pre-
vious section that green solvents could be prepared using both biogenic
as well as non-biogenic sources. Although green solvents could be eco-
nomically prepared using non-biogenic sources, but using such solvent
will diminish the objective of moving towards green solvents. The exist-
ing biogenic processes needs to be upgraded in a manner to make them
economical as like the petroleum based solvents to make them finan-
cially competitive. Efficacy of green solvents as compared to petroleum
based solvents is yet another area of concern. Although some studies
report higher extraction efficacy of green solvents, but otherwise re-
sults are also available. In addition, these extraction efficacy values are
prone to vary while up scaling the application of green solvents at the
industries scale. Practical situations have always shown that the labo-
ratory scale operating condition need to be adjusted again (to certain
extent) while up scaling the technology at the industrial/large scale. In
addition to this, the quality characteristics of the solvent extracted oil
may also be altered because of the differences in the polarity of green
solvent from the petroleum based solvents and the solubility of minor
constituents (polyphenols, vitamins, etc.) in the two. Also, the taste and
odour associated with green solvents (for example, ethyl acetate has
fruity odour, DMC has pleasant odour, etc.) is a challenge. Ethyl ac-
etate is present in certain products as a natural flavouring constituent.
For example, Cliff and Pickering (2006) reported that sensory panellists
were able to detect the perception of ethyl acetate in ice wine sample
at a concentration of 0.198 g/l. While, de la Roza et al. (2003) reported
that higher ethyl acetate concentration negatively affects the wine qual-
ity and imparts a shape acetic taste. Considering the volatile nature of
these solvents, it becomes very much essential to eliminate almost all of
the solvent residues from the extracted components. This is important
not only with regard to the inherent toxicity of the solvent but also to
avoid changes in the sensory properties of the solvent extracted prod-
uct. In addition to these, high working pressure and initial installation
cost required for the supercritical CO2 plant is also a major issue af-
fecting the up scaling supercritical extraction at the commercial scale
(Bubalo et al., 2018).
8. The way forward
Environment policies of international and national agencies are al-
ways emphasizing on the need to move from the petroleum based to-
wards renewable resources. The much discussed ‘global warming and
its consequences’ and increasing awareness of the common populace for
clean technologies have led to various researches in the field of green
chemistry, including green extraction. Solvent forms an important part
in the solvent extraction process. Issues pertaining to the environmental
impact and health hazard of conventionally used petroleum based sol-
vents have paved way for the search of alternative ‘green’ solvents which
tend to decrease the environmental pollution and are safe for the plant
operators as well as the consumers. Although, some reports are available
stating that green solvents could be used as an alternative to petroleum
based products in the food industry for extraction purpose, but they need
to be validated at larger (industrial) scale. Further, economic production
of green solvents is also cause of concern. While moving towards green
solvents, the aim should be to decrease the generation/use of hazardous
chemicals. Methodologies for production of green solvents should be
improved in a manner to make them economical as well as free from
the dependence/generation of hazardous chemicals. The quality char-
acteristics of products obtained using green solvents (like composition,
stability, residual solvent and associated toxicity, etc.) need to be stud-
ied and made at par with the conventionally available products obtained
using petroleum based products. At last but not the least, the findings
of green solvents should be spread to mass populace (including the ex-

10
W. Prasad, A.D. Wani, K. Khamrui et al.
traction industries and government agencies) to make them aware and
encourage them to move towards greener economy.
9. Conclusion
Solvent extraction has been used conventionally for isolation and
recovery of oil, flavouring compounds, anti-oxidants, etc. Easy and eco-
nomic availably of petroleum based solvents makes them the ideal
choice for commercial applications, however, their environmental and
health effects have emphasized on the search for alternative solvents.
Green solvents, a group of bio-based solvents having lower toxicity and
environmentally safe, are explored as a potential candidate for this. This
review included the studies pertaining to extraction efficacy of differ-
ent green solvents, viz., ethanol, di-methyl carbonate, ethyl acetate, 2-
MeTHF, etc. as a potential candidate for replacement of petroleum based
solvents during the solvent extraction process. Studies conducted us-
ing green solvents highlighted about their similar oil extraction efficacy
as that of their petroleum based counterparts. Industrial application of
green solvents will not only decrease the potential health hazards, but
also saves the environment by decreasing the emission of petroleum
based solvents and also by acting as means to economically utilize the
agricultural waste.
Declaration of competing interest
The authors have no conflict of interest to disclose with regard to
the present work.
CRediT authorship contribution statement
Writdhama Prasad: Conceptualization, Writing – original draft.
Aakash Dadarao Wani: Writing – original draft. Kaushik Khamrui:
Resources, Writing – review & editing. Shaik Abdul Hussain: Concep-
tualization, Writing – review & editing. Yogesh Khetra: Writing – re-
view & editing.
Data Availability Statement
Studies mentioned in this MS was derived from public domain re-
sources.
Acknowledgement
The authors are thankful to Director, ICAR-National Dairy Research
Institute, Karnal, Haryana for providing all the necessary facilities to
undertake this work. Also, the authors duly acknowledge the valuable
remarks provided by the Editor and Reviewers for improving the quality
of the paper.
References
Agata, T, 2017. Green solvents. J. Educ. Health Sport, 7, 224–232.
Ahmed, EH, Abadi, RS, Mohammed, AM, 2018. Phytochemical screening, chemical com-
position and antioxidant activity of seeds essential oil of Coriandrum sativum L. from
the Sudan. Int. J. Herbal Med. 6, 1–4.
Akintobi, O, Bamkefa, B, Adejuwon, A, Fagbbola, T, 2016. Phytochemical analysis and
antimicrobial evaluation of the extracts of the root bark and rachis of Parkia biglobosa
(Jacq). Benth on some human pathogens. E3 J. Sci. Res. 4, 1–10.
Akkol, EK, Goger, F, Koşar, M, Başer, KHC, 2008. Phenolic composition and biological ac-
tivities of Salvia halophila and Salvia virgata from Turkey. Food Chem. 108, 942–949.
Alliedmarketresearch.com. Internet document, https://www.alliedmarketresearch.com/
food-flavors-market, accessed on 04 Feb 2022.
Amarni, F, Kadi, H, 2010. Kinetics study of microwave-assisted solvent extraction of oil
from olive cake using hexane: comparison with the conventional extraction. Innovat.
Food Sci. Emerg. Technol. 11, 322–327.
Anastas, PT, Kirchhoff, MM, 2002. Origins, current status, and future challenges of green
chemistry. Acc. Chem. Res. 35, 686–694.
Anastas, PT, Williamson, T, 1996. In Green Chemistry: Designing Chemistry for the Envi-
ronment. ACS Symposium Series, pp. 1–17 Anastas, P. T., Williamson, T. (Eds.)626.
Anderson, S, 2019. Soxtec: its principles and applications. In: Oil Extraction and Analysis.
AOCS Publishing, pp. 11–24.
11
Cleaner Chemical Engineering 3 (2022) 100052
Aresta, M., Galatola, M., 1999. Life cycle analysis applied to the assessment of the en-
vironmental impact of alternative synthetic processes. The dimethylcarbonate case:
part 1. J. Clean. Prod. 7 (3), 181–193.
Awan, KA, Butt, MS, Ul Haq, I, Suleria, HA, 2019. Investigating the antioxidant potential
of garlic (Allium sativum) extracts through different extraction modes. Curr. Bioact.
Compd. 15 (1), 45–50.
Badola, R, Prasad, W, Panjagari, NR, Singh, RRB, Singh, AK, Hussain, SA, 2022. Khoa and
khoa based traditional dairy products: preparation, spoilage and shelf life extension.
J. Food Sci. Technol. 1–13.
Bimakr, M, Rahman, RA, Taip, FS, Ganjloo, A, Salleh, LM, Selamat, J, Zaidul, ISM, 2011.
Comparison of different extraction methods for the extraction of major bioactive
flavonoid compounds from spearmint (Mentha spicata L.) leaves. Food Bioprod. Pro-
cess. 89, 67–72.
Breil, C, Meullemiestre, A, Vian, M, Chemat, F, 2016. Bio-based solvents for green extrac-
tion of lipids from oleaginous yeast biomass for sustainable aviation biofuel. Molecules
21, 196. doi:10.3390/molecules21020196.
Bubalo, M.C., Vidović, S., Redovniković, I.R., Jokić, S., 2018. New perspective in extrac-
tion of plant biologically active compounds by green solvents. Food Bioprod. Process.
109, 52–73.
Capellini, MC, Giacomini, V, Cuevas, MS, Rodrigues, CEC, 2017. Rice bran oil extraction
using alcoholic solvents: Physicochemical characterization of oil and protein fraction
functionality. Ind. Crops Prod. 104, 133–143.
Castejón, N, Luna, P, Señoráns, FJ, 2018. Alternative oil extraction methods from Echium
plantagineum L. seeds using advanced techniques and green solvents. Food Chem.
244, 75–82.
Chemat, F., Abert Vian, M., Ravi, H.K., Khadhraoui, B., Hilali, S., Perino, S., Fabiano Tix-
ier, A.S., 2019. Review of alternative solvents for green extraction of food and natural
products: panorama, principles, applications and prospects. Molecules 24 (16), 3007.
doi:10.3390/molecules24163007.
Chen, Z., Shen, Q., Sun, N., Wei, W., 2019. Life cycle assessment of typical methanol
production routes: the environmental impacts analysis and power optimization. J.
Cleaner Prod. 220, 408–416.
Cheng, MH, 2017. Techno-economic analysis of soybean oil extruding-expelling process.
In: Cheng, M.H. (Ed.), Sustainability Analysis of Soybean Refinery: Soybean Oil Ex-
traction Process. Iowa State University, pp. 23–48 Ph.D. Dissertation.
Cheng, MH, Rosentrater, KA, 2017. Economic feasibility analysis of soybean oil production
by hexane extraction. Ind. Crops Prod. 108, 775–785.
Cheng, M.H., Sekhon, J.J., Rosentrater, K.A., Wang, T., Jung, S., Johnson, L.A., 2018. Envi-
ronmental impact assessment of soybean oil production: extruding-expelling process,
hexane extraction and aqueous extraction. Food Bioprod. Process. 108, 58–68.
Cliff, M.A., Pickering, G.J., 2006. Determination of odour detection thresholds for acetic
acid and ethyl acetate in ice wine. J. Wine Res. 17, 45–52.
Crinnion, WJ, 2010. The CDC fourth national report on human exposure to environmental
chemicals: what it tells us about our toxic burden and how it assists environmental
medicine physicians. Altern. Med. Rev. 15, 101–109.
de la Roza, C., Laca, A., Garcı́a, L.A., Dı́az, M., 2003. Ethanol and ethyl acetate production
during the cider fermentation from laboratory to industrial scale. Process Biochem.
38, 1451–1456.
Efeovbokhan, VE, Hymore, FK, Raji, D, Sanni, SE, 2015. Alternative solvents for Moringa
oleifera seeds extraction. J. Appl. Sci. 15, 1073–1082.
Eganathan, P, Subramanian, HS, Latha, R, Rao, CS, 2006. Oil analysis in seeds of Salicornia
brachiate. Ind. Crops Prod. 23, 177–179.
Esan, A.O., Adeyemi, A.D., Ganesan, S., 2020. A review on the recent application of
dimethyl carbonate in sustainable biodiesel production. J. Cleaner Prod. 257, 120561.
Fine, F, Vian, MA, Tixier, ASF, Carre, P, Pages, X, Chemat, F, 2013. Les agro-solvants
pour l’extraction des huiles végétales issues de graines oléagineuses. OCL 20, A502.
doi:10.1051/ocl/2013020.
Food Safety and Standards (Health Supplements, Nutraceuticals, Food for Spe-
cial Dietary Use, Food for Special Medical Purpose, Functional Food and
Novel Food) Regulations (2016). https://fssai.gov.in/upload/uploadfiles/files/FAQs_
Nutraceutical_Regulations_06_10_2020.pdf (accessed on 07/03/2022)
Fornasari, CH, Secco, D, Santos, RF, da Silva, TRB, Lenz, NBG, Tokura, LK, Gurgacz, F,
2017. Efficiency of the use of solvents in vegetable oil extraction at oleaginous crops.
Renew. Sustain. Energy Rev. 80, 121–124.
Gaber, MAFM, Tujillo, FJ, Mansour, MP, Juliano, P, 2018. Improving oil extraction from
canola seeds by conventional and advanced methods. Food Eng. Rev. 10, 198–210.
Gandhi, AP, Joshi, KC, Jha, K, Parihar, VS, Srivastav, DC, Raghunadh, P, Kawalker, J,
Jain, SK, Tripathi, RN, 2003. Studies on alternative solvents for the extraction of oil-I
soybean. Int. J. Food Sci. Technol. 38, 369–375.
Garba, U, Singanusong, R, Jiamyangyuen, S, Thongsook, T, 2017. Extraction and utiliza-
tion of rice bran oil: a review. In: The 4 th International Conference on Rice Bran
Oil Rice Bran Oil Application: Pharma-Cosmetics, Nutraceuticals and Foods, pp. 1–12
24-25 August 2017.
Garcia-Herrero, I., Cuéllar-Franca, R.M., Enriquez-Gutierrez, V.M., Alvarez-Guerra, M.,
Irabien, A., Azapagic, A., 2016. Environmental assessment of dimethyl carbonate pro-
duction: comparison of a novel electrosynthesis route utilizing CO2 with a commercial
oxidative carbonylation process. ACS Sustain. Chem. Eng. 4 (4), 2088–2097.
Gharby, S, Ravi, HK, Guillaume, D, Vian, MA, Chemat, F, Charrouf, Z, 2020. 2-methylox-
olane as alternative solvent for lipid extraction and its effect on the cactus (Opuntia
ficusindica L.) seed oil fractions. OCL 27, 1–7.
Gu, Y., Jerome, F., 2013. Bio-based solvents: an emerging generation of fluids for the
design of eco-efficient processes in catalysis and organic chemistry. Chem. Soc. Rev.
42, 9550–9570.
Häckl, K., Kunz, W., 2018. Some aspects of green solvents. C.R. Chim. 21, 572–580.
W. Prasad, A.D. Wani, K. Khamrui et al.
Hu, W, Wells, JH, Shin, TS, Godber, JS, 1996. Comparison of isopropanol and hexane for
extraction of vitamin E and oryzanols from stabilized rice bran. J. Am. Oil Chemists’
Soc. 73, 1653–1656.
Johnson, LA, Lusas, EW, 1983. Comparison of alternative solvents for oil extraction. J.
Am. Oil Chemists’ Soc. 60, 229–241.
Jutz, F, Adanson, JM, Balker, A, 2011. Ionic liquids and dense carbon dioxide: a beneficial
biphasic system for catalysis. Chem. Rev. 111, 322–353.
Kanadea, R, Bhatkhandeb, DS, 2016. Extraction of ginger oil using different methods and
effect of solvents, time, temperature to maximize yield. Int. J. Adv. Sci. Eng. Technol.
4, 241–244.
Kumar, SJ, Prasad, SR, Banerjee, R, Agarwal, DK, Kulkarni, KS, Ramesh, KV, 2017. Green
solvents and technologies for oil extraction from oilseeds. Chem. Cent. J. 11, 1–7.
Kumbhare, S, Prasad, W, Khamrui, K, Wani, AD, Sahu, J, 2021. Recent innovations in
functionality and shelf life enhancement of ghee, clarified butter fat. J. Food Sci.
Technol. 1–13.
Lakkakula, NR, Lima, M, Walker, T, 2004. Rice bran stabilization and rice bran oil extrac-
tion using ohmic heating. Bioresour. Technol. 92, 157–161.
Logsdon, JE, Loke, RA, 2000. Isopropyl alcohol. Kirk-Othmer Encycl. Chem. Technol.
doi:10.1002/0471238961.0919151612150719.a01.
Lohani, UC, Fallahi, P, Muthukumarappan, K, 2015. Comparison of ethyl acetate with
hexane for oil extraction from various oilseeds. J. Am. Oil Chem. Soc. 92, 743–754.
Meena, S, Prasad, W, Khamrui, K, Mandal, S, Bhat, S, 2021a. Preparation of spray-dried
curcumin microcapsules using a blend of whey protein with maltodextrin and gum
arabica and its in-vitro digestibility evaluation. Food Biosci. 41, 100990.
Meena, S., Gote, S., Prasad, W., Khamrui, K., 2021b. Storage stability of spray dried cur-
cumin encapsulate prepared using a blend of whey protein, maltodextrin, and gum
Arabic. J. Food Process. Preserv. 45 (5), e15472.
Miller, KG, Poole, CF, Chichila, TMP, 1995. Solvent – assisted supercritical fluid extrac-
tion for the isolation of semi-volatile flavour compounds from the cinnamons of com-
merce and their separation by series-coupled column. J. High-Resolut. Chromatogr.
18, 461–471.
Mohammadpour, H, Sadrameli, SM, Eslami, F, Asoodeh, A, 2019. Optimization of ultra-
sound-assisted extraction of Moringa peregrina oil with response surface methodology
and comparison with Soxhlet method. Ind. Crops Prod. 131, 106–116.
Molnar, M, Mendesevic, N, Subaric, D, Banjari, I, Jokic, S, 2017. Comparison of various
techniques for the extraction of umbelliferone and herniarin in Matricaria chamomilla
processing fractions. Chem. Cent. J. 11, 1–8.
Monsálvez, M, Zapata, N, Vargas, M, Berti, M, Bittner, M, Hernández, V, 2010. Antifungal
effects of n-hexane extract and essential oil of Drimys winteri bark against Take-All
disease. Ind. Crops Prod. 31, 239–244.
Moreau, RA, Powell, MJ, Singh, V, 2003. Pressurized liquid extraction of polar and nonpo-
lar lipids in corn and oats with hexane, methylene chloride, isopropanol, and ethanol.
J. Am. Oil Chem. Soc. 80, 1063–1067.
Naik, M, Natarajan, V, Rawson, A, Rangarajan, J, Manickam, L, 2021. Extraction kinetics
and quality evaluation of oil extracted from bitter gourd (Momardica charantia L.)
seeds using emergent technologies. LWT 140, 110714.
Oliveira, R, Oliveira, V, Aracava, KK, da Costa Rodrigues, CE, 2012. Effects of the extrac-
tion conditions on the yield and composition of rice bran oil extracted with ethanol—a
response surface approach. Food Bioprod. Process. 90, 22–31.
Pace, V, Hoyos, P, Castoldi, L, Dominguez de Maria, P, Alcántara, AR, 2012. 2-Methyl-
tetrahydrofuran (2-MeTHF): a biomass-derived solvent with broad application in or-
ganic chemistry. ChemSusChem 5, 1369–1379.
Peev, GP, Penchev, D, Peshev, Angelov G, 2011. Solvent extraction of rosmarinic acid from
lemon balm and concentration of extracts by nanofiltration: Effect of plant pre-treat-
ment by supercritical carbon dioxide. Chem. Eng. Res. Des. 89, 2236–2243.
Perrier, A, Delsart, C, Boussetta, N, Grimi, N, Citeau, M, Vorobiev, E, 2017. Effect of
ultrasound and green solvents addition on the oil extraction efficiency from rapeseed
flakes. Ultrason. Sonochem. 39, 58–65.
Pinto, JSS, Nixdorf, SL, Sinisterra, MJ, Lanças, FM, 2019. A novel coffee oil extraction
procedure employing pressurized solvents. Scientia Chromatographica 11, 28–33.
Potrich, E., Miyoshi, S.C., Machado, P.F., Furlan, F.F., Ribeiro, M.P., Tardioli, P.W., …
Giordano, R.C., 2020. Replacing hexane by ethanol for soybean oil extraction: Model-
ing, simulation, and techno-economic-environmental analysis. J. Cleaner Prod. 244,
118660.
12
Cleaner Chemical Engineering 3 (2022) 100052
Ravi, HK, Vian, MA, Tao, Y, Degrou, A, Costil, J, Trespeuch, C, Chemat, F, 2019. Alter-
native solvents for lipid extraction and their effect on protein quality in black soldier
fly (Hermetia illucens) larvae. J. Cleaner Prod. 238, 117861.
Rose, A, Jaczynski, J, Matak, K, 2021. Extraction of lipids from insect powders using a
one-step organic solvent extraction process. Future Foods 4, 100073.
Sandhya, S, Khamrui, K, Prasad, W, Kumar, MCT, 2018. Preparation of pomegranate peel
extract powder and evaluation of its effect on functional properties and shelf life of
curd. LWT 92, 416–421.
Saponjac, VT, Cetojevic-Simin, D, Cetkovic, G, Canadanovic-Brunet, J, Djilas, S, Mandic, A,
Tepic, A, 2014. Effect of extraction conditions of paprika oleoresins on their free rad-
ical scavenging and anticancer activity. Cent. Eur. J. Chem. 12, 377–385.
Saxena, DK, Sambi, SS, Sharma, SK, 2011. Comparative extraction of cottonseed oil by
n-Hexane and Ethanol. J. Eng. Appl. Sci. 6, 84–89.
Sicaire, AG, Vian, M, Fine, F, Joffre, F, Carré, P, Tostain, S, Chemat, F, 2015. Alternative
bio-based solvents for extraction of fat and oils: solubility prediction, global yield,
extraction kinetics, chemical composition and cost of manufacturing. Int. J. Mol. Sci.
16, 8430–8453.
Siddique, MAB, Tzima, K, Rai, DK, Brunton, N, 2020. Conventional Extraction Techniques
for Bioactive Compounds from Herbs and Spices. In: Herbs, Spices and Medicinal
Plants: Processing, Health Benefits and Safety, pp. 69–93.
Slater, CS, Savelski, MJ, Hitchcock, D, Cavanagh, EJ, 2016. Environmental analysis of the
life cycle emissions of 2-methyl tetrahydrofuran solvent manufactured from renew-
able resources. J. Environ. Sci. Health, Part A, 51, 487–494.
Te, KGD, Go, AW, Wang, HJD, Guevarra, RG, Cabatingan, LK, Tabanag, IDF, Ju, YH, 2020.
Extraction of lipids from post-hydrolysis copra cake with hexane as solvent: Kinetic
and equilibrium data. Renew. Energy 158, 311–323.
Torgbo, S, Sukatta, U, Kamonpatana, P, Sukyai, P, 2022. Ohmic heating extraction and
characterization of rambutan (Nephelium lappaceum L.) peel extract with enhanced
antioxidant and antifungal activity as a bioactive and functional ingredient in white
bread preparation. Food Chem., 132332.
Umamaheshwari, P, Reddy, PDS, 2016. Effect of operating parameters on extraction of
oil from bitter gourd seeds: A kinetic and thermodynamic study. Int. J. Sci. Res. 5,
1243–1246.
Vagi, E, Rapavi, E, Hadolin, M, Vasarhelyine Peredi, K, Balazs, A, Blazovics, A, Simandi, B,
2005. Phenolic and triterpenoid antioxidants from Origanum majorana L. herb and
extracts obtained with different solvents. J. Agric. Food Chem. 53, 17–21.
Wani, AD, Prasad, W, Khamrui, K, Jamb, S, 2022a. A review on quality attributes and
utilization of ghee residue, an under-utilized dairy by-product. Future Foods, 100131
doi:10.1016/j.fufo.2022.100131.
Wani, AD, Prasad, WG, Khamrui, K, Hussain, SA, Deep, A, 2022b. Evaluation of green sol-
vent as an environment friendly alternative for milk fat extraction from ghee residue
(clarified butter sediment waste). Int. J. Food Sci. Technol. doi:10.1111/ijfs.15967.
Watanabe, K, Yamagiwa, N, Torisawa, Y, 2007. Cyclopentyl methyl ether as a new and
alternative process solvent. Org. Process Res. Dev. 11, 251–258.
Ying, Li, Frederic, Fine, Anne-Sylvie, Fabiano-Tixier, Maryline, Abert-Vian, Patrick, Carre,
Xavier, Pages, Farid, Chemat, 2013. Evaluation of alternative solvents for improve-
ment of oil extraction from rapeseeds. C.R. Chim. 17, 242–251.
Zhang, F, Rhee, KC, Koseoglu, SS, 2002. Isopropyl alcohol extraction of cottonseed collets:
efficiency and performance. J. Food Lipids 9, 147–160.
Zhimin, Xu, Samuel Godber, J, 2000. Comparison of supercritical fluid and solvent ex-
traction methods in extracting 𝛾-oryzanol from rice bran. J. Am. Oil Chem. Soc. 77,
547–551.
Zhou, B, Gao, X, Liu, Q, Chen, Y, Zhang, D, 2019. Trace Component Characteristic of
Petroleum Ether Extracts from Different Camellia Seed Oil Products. Ekoloji 28,
81–86.
Zhuang, X, Zhang, Z, Wang, Y, Li, Y, 2018. The effect of alternative solvents to n-hexane
on the green extraction of Litsea cubeba kernel oils as new oil sources. Ind. Crops
Prod. 126, 340–346.
Ziaedini, A, Jafari, A, Zakeri, A, 2010. Extraction of antioxidants and caffeine from
green tea (Camelia sinensis) leaves: kinetics and Modeling. Food Sci. Technol. Int. 16,
505–510.